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1.
    
Molecular dynamics and related atomistic computer simulations are effective ways in studying the structures and structure–property relations of glass materials. However, simulations of boron oxide (B2O3)-containing oxide glasses pose a challenge due to the lack of reliable empirical potentials. This paper reports development of a set of partial charge pairwise composition-dependent potentials for boron-related interactions that enable simulations of multicomponent borosilicate glasses, together with some of the existing parameters. This set of potentials was tested in sodium borate glasses and sodium borosilicate glasses and it is shown capable to describe boron coordination change with glass composition in wide composition ranges. Structure features such as boron N4 value, density, Qn species distribution, fraction of non-bridging oxygen around boron and silicon, total correlation function, and bond angle distribution function were calculated and compared with available experimental data. Mechanical properties of the simulated glasses calculated with the new potential also show good agreement with experiments. Therefore, this new set of potential can be used to simulate boron oxide-containing multicomponent glasses including those with wide industrial and technology applications.  相似文献   

2.
    
Borates and borosilicates are potential candidates for the design and development of glass formulations with important industrial and technological applications. A major challenge that retards the pace of development of borate/borosilicate based glasses using predictive modeling is the lack of reliable computational models to predict the structure-property relationships in these glasses over a wide compositional space. A major hindrance in this pursuit has been the complexity of boron-oxygen bonding due to which it has been difficult to develop adequate B–O interatomic potentials. In this article, we have evaluated the performance of three B–O interatomic potential models recently developed by Bauchy et al [J. Non-Cryst. Solids, 2018, 498, 294–304], Du et al [J. Am. Ceram. Soc. https://doi.org/10.1111/jace.16082 ] and Edèn et al [Phys. Chem. Chem. Phys., 2018, 20, 8192–8209] aiming to reproduce the short-to-medium range structures of sodium borosilicate glasses in the system 25 Na2O x B2O3 (75 − x) SiO2 (x = 0-75 mol%). To evaluate the different force fields, we have computed at the density functional theory level the NMR parameters of 11B, 23Na, and 29Si of the models generated with the three potentials and the simulated MAS NMR spectra compared with the experimental counterparts. It was observed that the rigid ionic models proposed by Bauchy and Du can both reliably reproduce the partitioning between BO3 and BO4 species of the investigated glasses, along with the local environment around sodium in the glass structure. However, they do not accurately reproduce the second coordination sphere of silicon ions and the Si–O–T (T = Si, B) and B-O-T distribution angles in the investigated compositional space which strongly affect the NMR parameters and final spectral shape. On the other hand, the core-shell parameterization model proposed by Edén underestimates the fraction of BO4 species of the glass with composition 25Na2O 18.4B2O3 56.6SiO2 but can accurately reproduce the shape of the 11B and 29Si MAS-NMR spectra of the glasses investigations due to the narrower B–O–T and Si-O-T bond angle distributions. Finally, the effect of the number of boron atoms (also distinguishing the BO3 and BO4 units) in the second coordination sphere of the network former cations on the NMR parameters have been evaluated.  相似文献   

3.
    
Borosilicate glasses incorporating high-level nuclear waste are exposed to high-energy radiations during their storage in the deep geological repositories. However, the effect of radiation on the atomic structure of borosilicate glasses remains poorly understood. Herein, using molecular dynamics simulations, we study the irradiation-induced structural changes of a series of calcium-sodium borosilicate glasses with varying Si/B molar ratios—ranging from pure silicate to pure borate glasses. We observe that irradiation leads to an increase in disorder, both in the short- and medium-range, as evidenced by the enthalpy, coordination number, and ring distribution. In particular, the impact of the change in the atomic structure (due to radiation) on the glass volume is investigated. Interestingly, we observe a composition-dependent transition in the volumetric response of borosilicate glasses under irradiation—wherein borate-rich compositions tend to swell, whereas silica-rich glasses tend to densify. Through a detailed analysis of the structure, we demonstrate two competing mechanisms contributing to the volume change, i.e., a decrease in the coordination number of boron atoms and a reduction in the average silicon inter-polytope angle. We also show that the increase in the disorder in the medium-range order may play a major role in governing the volumetric changes in the irradiated structure in a non-trivial fashion. Altogether, the present study highlights that irradiation has a non-trivial effect on borosilicate glasses, which, in turn, could impact their corrosion kinetics.  相似文献   

4.
    
In this study, hot-compression is applied to two multicomponent borosilicate glasses, Borofloat33 (Boro33) and N-BK7, using molecular dynamics simulations. The effects of pressure on elastic properties, surface energy, and fracture toughness ( are investigated. It is found that the impact on is mainly dominated by the change of Young's modulus under pressure, which is proportional to the relative change in density. Between the two glasses under investigation, can be improved more effectively by the hot-compression process for Boro33, due to its higher concentration of 3-coordinated boron (B3), which facilitates densification via B3 to B4 conversion under compression.  相似文献   

5.
Surface plays an important role in the physical and chemical properties of oxide glasses and controls the interactions of these glasses with the environment, thus dominating properties such as the chemical durability and bioactivity. The surface atomic structures of a series of sodium borosilicate glasses were studied using classical molecular dynamics simulations with recently developed compositional dependent partial charge potentials. The surface structural features and defect speciation were characterized and compared with the bulk glasses with the same composition. Our simulation results show that the borosilicate glass surfaces have significantly different chemical compositions and structures as compared to the bulk. The glass surfaces are found to be sodium enriched and behave like borosilicate glasses with higher R (Na2O/B2O3) values. As a result of this composition and associated structure changes, the amount of fourfold boron decreases at the surface and the network connectivity on the surface decreases. In addition to composition variation and local structure environment change, defects such as two‐membered rings and three‐coordinated silicon were also observed on the surface. These unusual surface composition and structure features are expected to significantly impact the chemical and physical properties and the interactions with the environments of sodium borosilicate glasses.  相似文献   

6.
A modified associate species approach is used to model the liquid phase in oxide systems. The relatively simple technique treats oxide liquids as solutions of end-member and associate species. The model is extended to representing glasses by treating them as undercooled liquids. Equilibrium calculations using the model allow the determination of species activities, phase separation, precipitation of crystalline phases, and volatilization. In support of nuclear waste glass development, a model of the Na2O–Al2O3–B2O3–SiO2 system has been developed that accurately reproduces its phase equilibria. The technique has been applied to the CaO–SiO2 system, which is used to demonstrate how two immiscible liquids can be treated.  相似文献   

7.
    
Classical molecular dynamics simulations have been used to investigate the structural role of Mg and its effect when it is incorporated in sodium aluminoborosilicate glasses. The simulations have been performed using three interatomic potentials; one is based on the rigid ionic model parameterized by Wang et al. (2018) and two slightly different parameterization of the core–shell model provided by Stevensson et al. (2018) and Pedone et al. (2020) The accuracies of these models have been assessed by detailed structural analysis and comparing the simulated nuclear magnetic resonance (NMR) spectra for spin active nuclei (29Si, 27Al, 11B, 17O, 25Mg, and 23Na) with the experimental counterparts collected in a previous work. Our simulations reveal that the core–shell parameterizations provide better structural models. In fact, they better reproduce the NMR spectra of all the investigated nuclei and give better agreement with known experimental data. Magnesium is found to be five coordinated on average with distances with oxygen in between a network modifier (like Na) and an intermediate network formed (like Al). It prefers to lay closer to three-coordinated B atoms, forming B–NBO bonds, with respect to Si and especially Al. This can explain the formation of AlO5 and AlO6 units in the investigated Na-free glass, together with a Si clusterization.  相似文献   

8.
    
High-alumina containing high-level waste (HLW) will be vitrified at the Waste Treatment Plant at the Hanford Site. The resulting glasses, high in alumina, will have distinct composition-structure-property (C-S-P) relationships compared to previously studied HLW glasses. These C-S-P relationships determine the processability and product durability of glasses and therefore must be understood. The main purpose of this study is to understand the detailed structural changes caused by Al:Si and (Al + Na):Si substitutions in a simplified nuclear waste model glass (ISG, international simple glass) by combining experimental structural characterizations and molecular dynamics (MD) simulations. The structures of these two series of glasses were characterized by neutron total scattering and 27Al, 23Na, 29Si, and 11B solid-state nuclear magnetic resonance (NMR) spectroscopy. Additionally, MD simulations were used to generate atomistic structural models of the borosilicate glasses and simulation results were validated by the experimental structural data. Short-range (eg, bond distance, coordination number, etc) and medium-range (eg, oxygen speciation, network connectivity, polyhedral linkages) structural features of the borosilicate glasses were systematically investigated as a function of the degree of substitution. The results show that bond distance and coordination number of the cation-oxygen pairs are relatively insensitive to Al:Si and (Al + Na):Si substitutions with the exception of the B-O pair. Additionally, the Al:Si substitution results in an increase in tri-bridging oxygen species, whereas (Al + Na):Si substitution creates nonbridging oxygen species. Charge compensator preferences were found for Si-[NBO] (Na+), [3]B-[NBO] (Na+), [4]B (mostly Ca2+), [4]Al (nearly equally split Na+ and Ca2+), and [6]Zr (mostly Ca2+). The network former-BO-network former linkages preferences were also tabulated; Si-O-Al and Al-O-Al were preferred at the expense of lower Si-O-[3]B and [3]B-O-[3]B linkages. These results provide insights on the structural origins of property changes such as glass-transition temperature caused by the substitutions, providing a basis for future improvements of theoretical and computer simulation models.  相似文献   

9.
    
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10.
    
The mechanical response of multicomponent borosilicate glasses has drawn significant attention in the design of damage-resistant glasses. In this work, we investigate the plasticity of two borosilicate glasses, Borofloat®33 (Boro33) and N-BK7®, by implementing a uniaxial tension test using molecular dynamics simulations. A bond-switching mechanism is found to be responsible for the plastic response of both glasses and is governed by the increasing rate of non-bridging oxygen (NBO) production during the uniaxial tension. We found that the amount of B4OSi4 linkages in the glass governs the stress drop after yielding, due to its higher tendency to create NBOs compared to Si4OSi4. Also, the initial existence of NBOs weakens the critical stress for breaking the B4-O bond in B4OSi4, which in turn lowers the yield strength of the glass. The local atomic constraints are analyzed in the two glasses, and high anti-correlation between the concentration of rigid constraints and plastic deformation is observed.  相似文献   

11.
硼硅酸盐玻璃鳞片研制开发概况   总被引：1，自引：0，他引：1  
许求鑫 《上海涂料》2002,40(4):8-10
叙述了我国玻璃鳞片的研究和开发历程,提出了厚度和表面处理的重要性。  相似文献   

12.
宁红兵 《玻璃》2012,39(8):3-5
介绍了全氧燃烧技术的特点和高硼硅玻璃的生产现状,探讨了全氧燃烧高硼硅浮法玻璃窑炉的结构特点,指出了全氧燃烧技术在高技术玻璃生产上的应用前景。  相似文献   

13.
The study of the bond breaking and formation processes, that is, the chemical reaction, in the Si–O network structure in liquid alkali silicates at temperatures around or higher than the glass-transition temperature is important for understanding kinetic processes such as the structural relaxation of the network, viscous flow, and diffusion of the network former ions. Herein, novel methods for analyzing the reactions in a molecular-dynamics-modeled liquid Na2SiO3 were used to confirm the following results: (a) the substitutional reactions (in which a nonbridging O ion of a Si–O chain or a SiO4 tetrahedron attacks the Si ion of another chain from backside of a bridging O ion, which acts as the leaving group, and the bridging O leaves the Si ion) primarily occur in the Si–O network of liquid Na2SiO3; and (b) The abundance ratio of Qn species can be quantitatively reproduced by the reaction rate.  相似文献   

14.
范正明 《化工设计》2001,11(5):15-16,21
介绍硼硅玻璃管道的性能、特点和应用情况;阐述其安装方法及其注意事项。  相似文献   

15.
低温烧结硼硅钙复相微晶玻璃的结构和性能   总被引：1，自引：0，他引：1  
在硼硅钙(CaO-B2O3-SiO2, CBS)玻璃中添加硼硅酸玻璃,低温烧结制备了CBS复相微晶玻璃.研究了硼硅酸玻璃的添量及烧成温度对CBS复相微晶玻璃性能的影响规律.用X射线衍射和扫描电镜微观结构分析方法研究了材料性能与结构的关系.结果表明:硼硅酸玻璃与CBS玻璃具有很好的相容性,硼硅酸玻璃的质量分数(下同)为10%～40%的范围内均可在850℃烧结.随着硼硅酸玻璃的引入,样品中生成了具有低相对介电常数(εr)和高热膨胀系数(α)的α-石英.硼硅酸玻璃有效降低了材料的εr,实现了εr在5.6～6.6范围内可调.硼硅酸玻璃的添量小于20%时,α增加幅度较小,随着硼硅玻璃添量进一步增加(30%～40%),α显著增大.烧成温度的升高可促使玻璃中晶体析出和长大且析出晶相具有比CBS玻璃低的εr,样品的εr随着烧成温度的升高呈下降趋势.  相似文献   

16.
    
The glass transition temperature (Tg) is a key parameter to investigate for application in nuclear waste immobilization in borosilicate glasses. Tg for several glasses containing iodine (I) has been measured in order to determine the I effect on Tg. Two series of glass composition (ISG and NH) containing up to 2.5 mol% I and synthesized under high pressure (0.5 to 1.5 GPa) have been investigated using differential scanning calorimetry (DSC). The I local environment in glasses has been determined using X-ray photoelectron spectroscopy and revealed that I is dissolved under its iodide form (I−). Results show that Tg is decreased with the I addition in the glass in agreement with previous results. We also observed that this Tg decrease is a strong function of glass composition. For NH, 2.5 mol% I induces a decrease of 24°C in Tg, whereas for ISG, 1.2 mol% decreases the Tg by 64°C. We interpret this difference as the result of the I dissolution mechanism and its effect on the polymerization of the boron network. The I dissolution in ISG is accompanied by a depolymerization of the boron network, whereas it is the opposite in NH. Although ISG corresponds to a standardized glass, for the particular case of I immobilization it appears less adequate than NH considering that the decrease in Tg for NH is small in comparison to ISG.  相似文献   

17.
    
Knowledge of the underlying structural response during deformation processes is essential for understanding the macroscopic mechanical response of glass. Here we present results from cold compression-decompression molecular dynamics (MD) simulations of two multicomponent borosilicate glasses, Borofloat®33 (Boro33) and N-BK7® (N-BK7). Our results suggest that the densification of these two borosilicate glasses involves different types of structural changes. The fraction of permanent densification can be correlated to the change in intermediate-range structure. By performing Voronoi analysis, we quantify the contributions to densification from different cation types in these two multicomponent borosilicate glasses, finding that 3-coordinated cations facilitate the densification process. Higher-coordinated cations are relatively stable and can even show a slight expansion in their Voronoi volume.  相似文献   

18.
    
One of the key factors, which hampers the application of metallic glasses as structural components, is the localization of deformation in narrow bands of a few tens up to one hundred nanometers thickness, the so-called shear bands. Processes, which occur inside shear bands are of central importance for the question whether a catastrophic failure of the material is unavoidable or can be circumvented or, at least, delayed. Via molecular dynamics simulations, this study addresses one of these processes, namely the local temperature rise due to viscous heat generation. The major contribution to energy dissipation is traced back to the plastic work performed by shear stress during steady deformation. Zones of largest strain contribute the most to this process and coincide with high-temperature domains (hottest spots) inside the sample. Magnitude of temperature rise can reach a few percent of the sample’s glass transition temperature. Consequences of these observations are discussed in the context of the current research in the field.  相似文献   

19.
    
Bioactive glass coatings can improve the osteo integration of metallic implants with the host tissue, thereby increasing their lifespan and overall success rate. However, complex composition-structure-property relations in phosphosilicate-based bioactive glasses make experimental determination of these relations and related composition design of bioactive coatings challenging. By applying molecular dynamics (MD)-based atomistic simulations with recently developed effective potentials, this work addresses the challenge by using a material genome approach to obtain the composition and structure effects on various key properties for bioactive coating applications. A series of potential bioactive glass compositions were studied and the composition effects on the mechanical and thermal properties that are critical to these bioactive glasses as a coating to metallic implants were calculated. Particularly, by varying the level of B2O3 to SiO2 substitutions, the effect of composition on various key properties was elucidated. It was found that by using cation in a 1 to 1 ratio (BO3/2 to SiO2) instead of the commonly used substitutions (B2O3 to SiO2), the composition effect can be more clearly expressed and, hence, recommended in future composition designs. Together with careful structural analysis, the origin of property changes can be elucidated. The atomistic computer simulation-based approach is, thus, an effective way to guide future bioactive glass designs for bioactive coatings and other applications.  相似文献   

20.
    
The thermal stability of sol-gel-derived silica and borosilicate glasses exposed to dry O2 at 800 and 1200°C for 100 hours was characterized by weight change, thermal transitions, morphology, structure, and composition to investigate suitability as models for thermally grown oxides. Rapid weight loss was observed in the first few hours of isothermal exposure for borosilicate glasses, followed by constant weight loss at a low rate for the balance of the exposure. Weight loss resulted from loss of residual hydroxyl species retained from the sol-gel synthesis, and from oxidation of carbon retained from thermal decomposition of the organic precursors by pyrolysis. Characterization of the sol-gel-derived glasses showed structural similarities to silica and binary borosilicate glasses synthesized by melt or vapor deposition methods, and to thermally grown oxides. Oxygen transport mechanisms through the sol-gel-derived glasses is not thought to be affected by the retained carbon. However, a silica-enriched glass surface resulting from boria volatility, observed from a borosilicate glass exposed dry O2 at 1200°C, will slow O2 transport rates. The results show that sol-gel-derived silica and borosilicate glasses can be used as models for thermally grown oxides.  相似文献   

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